Ni/Mg–Al catalysts derived from hydrotalcite-type precursors were prepared by a co-precipitation technique and applied to steam reforming of methane. By comparison with Ni/γ-Al2O3 and Ni/α-Al2O3 catalysts prepared ...Ni/Mg–Al catalysts derived from hydrotalcite-type precursors were prepared by a co-precipitation technique and applied to steam reforming of methane. By comparison with Ni/γ-Al2O3 and Ni/α-Al2O3 catalysts prepared by incipient wetness impregnation, the Ni/Mg–Al catalyst presented much higher activity as a result of higher specific surface area and better Ni dispersion. The Ni/Mg–Al catalyst with a Ni/Mg/Al molar ratio of 0.5:2.5:1 exhibited the highest activity for steam methane reforming and was selected for kinetic investigation. With external and internal diffusion limitations eliminated, kinetic experiments were carried out at atmospheric pressure and over a temperature range of 823–973 K. The results demonstrated that the overall conversion of CH4 and the conversion of CH4 to CO2were strongly influenced by reaction temperature, residence time of reactants as well as molar ratio of steam to methane. A classical Langmuir–Hinshelwood kinetic model proposed by Xu and Froment(1989)fitted the experimental data with excellent agreement. The estimated adsorption parameters were consistent thermodynamically.展开更多
Adsorption equilibrium isotherms of benzene in the concentrationrange of 500-4000 mg·m^-3 on two commercial activated carbons wereobtained using long-column method under 30 deg. C and differenthumidity condi- tio...Adsorption equilibrium isotherms of benzene in the concentrationrange of 500-4000 mg·m^-3 on two commercial activated carbons wereobtained using long-column method under 30 deg. C and differenthumidity condi- tions. Results show that the benzene and water vaporshave depression effects upon the adsorption of each other and thatthe unfavorable effect of water vapor resembles its single-componentisotherm on activated carbon. A com- petitive adsorption model wasproposed to explore the depression mechanisms of the non-ideal,non-similar binary adsorption systems.展开更多
We synthesized a mesoporous film based on TiO2-reduced graphene oxide(RGO)hybrids using a one-step vapor-thermal method without the need for an additional annealing process.The vapor-thermally prepared TiO2-graphene h...We synthesized a mesoporous film based on TiO2-reduced graphene oxide(RGO)hybrids using a one-step vapor-thermal method without the need for an additional annealing process.The vapor-thermally prepared TiO2-graphene hybrid(VTH)features unique structures with an ultra-large specific surface area of^260 m^2 g^-1 and low aggregation,giving rise to enhanced light harvesting and increased charge generation and separation efficiency.It was observed that a mesoporous film with uniform pore distribution is simultaneously obtained during the VTH growth process.When a 5.0 wt%RGO VTH film was used as the active layer in photocatalysis,the highest photocatalytic activity for degradation of methyl orange was achieved.For another,when a 0.75 wt%RGO VTH film was used as the photoanode in a dye-sensitized solar cell,the power conversion efficiency reached 7.58%,which represents an increase of 73.1%compared to a solar cell using an a photoanode of pure TiO2 synthesized by a traditional solvothermal method.It is expected that this facile method for the synthesis of TiO2/graphene hybrid mesoporous films will be useful in practical applications for preparing other metal oxide/graphene hybrids with ultra-high photocatalytic activity and photovoltaic performance.展开更多
A simplified model was developed to describe the water vapor adsorption on activated carbon. The development of the simplified model was started from the original model proposed by DO and his co-workers. Two different...A simplified model was developed to describe the water vapor adsorption on activated carbon. The development of the simplified model was started from the original model proposed by DO and his co-workers. Two different kinds of carbon materials were prepared for water vapor adsorption, and the adsorption experiments were conducted at different temperatures(20-50 °C) and relative humidities(5%-99%) to test the model. It is shown that the amount of adsorbed water vapor in micropore decreases with the temperature increasing, and the water molecules form larger water clusters around the functional group as the temperature is up to a higher value. The simplified model describes reasonably well for all the experimental data. According to the fitted values, the parameters of simplified model were represented by the temperature and then the model was used to calculate the water vapor adsorption amount at 25 °C and 35 °C. The results show that the model can get relatively accurate values to calculate the water vapor adsorption on activated carbon.展开更多
The XG equation, which is developed by us previously for describing the adsorption equilibrium of pure vapor on activated carbon, is extended to multi-component system. Verified by experimental data, the extended XG e...The XG equation, which is developed by us previously for describing the adsorption equilibrium of pure vapor on activated carbon, is extended to multi-component system. Verified by experimental data, the extended XG equation was found to be more successful in predicting the adsorption equilibrium of vapor mixture on activated carbon than the extended Langmuir equation, the extended BET equation and the ideal adsorbed solution theory (IAST).展开更多
This study was conducted to evaluate the effect of different distillation methods of Mentha cordifolia Opiz. essential oil on antibacterial activity. The essential oils were isolated by water and steam, hydro, ethanol...This study was conducted to evaluate the effect of different distillation methods of Mentha cordifolia Opiz. essential oil on antibacterial activity. The essential oils were isolated by water and steam, hydro, ethanol, and 3methanol： lethanol distillations. Moreover, we also compared the efficacy of these various distillations with commercial peppermint oil. Essential oils were tested in vitro against three pathogen bacteria species by sensitivity test include disc diffusion assay （DD）, minimal inhibition concentration （MIC） and maximal bactericidal concentration （MBC）. Escherichia coli, Staphylococcus aureus and Salmonella typhimurium were used in this investigation. The results showed that the water and steam distillation and 3methanol： lethanol under tested by DD assay was found to be effective against all the pathogenic bacteria, in which the zone of inhibition exhibited E. coil S. aureus and S. typhimurium were 9.67 ± 0.35, 11.67 ± 0.66, 18.0± 1.15 and 9.00 ± 0.05, 8.3 ± 0.35, 19.0 ± 0.00 ram, respectively. While the hydro and ethanol distillations did action to against only E. coli which the inhibition zones were 8.67 ± 0.66 and 8.67 ± 0.35 mm, respectively. However, the commercial oil was more effective against tested pathogenic bacteria than all M. cordifolia essential oil. In case of MIC and MBC assays, the results showed that all essential oil distillation methods posed antibacterial potential in which the water and steam distillation showed the lowest MIC and MBC values against E. coli, S. aureus and S. typhimurium. It is suggested that among all M. cordifolia essential oil extractions, water and steam distillation was found to be highly bactericidal as it has shown in lowest MIC and MBC values and high in growth inhibition zone diameter.展开更多
Five different kinds of hydrophilic organic salts were used to modify commercial activated carbon in order to prepare hydrophilic carbon materials. Properties of the samples were analyzed by surface area analyzer and ...Five different kinds of hydrophilic organic salts were used to modify commercial activated carbon in order to prepare hydrophilic carbon materials. Properties of the samples were analyzed by surface area analyzer and SEM-EDX. The hydrophilic organic salts with different properties were introduced into activated carbon and significantly affected the properties of the samples.During adsorption experiments, the water vapor adsorption amount in modified samples increases by 0.57-17.12 times in temperature range from 303 to 323 K and at relative pressure below 0.50. Water molecules combined with surface hydrophilic groups through H-bonding exhibit good thermo stability. The effects of temperature, oxygen content and properties of the hydrophilic organic salts on water vapor adsorption were studied. It is indicated that water vapor adsorption in modified samples is mainly affected by the surface oxygen content. The carboxylate radicals in the hydrophilic organic salts greatly affect the micropore structure of the modified samples, while the metal ions in them exhibit limited influence. Different adsorption capacity of modified samples can be explained with the electronegativity of elements presented by Pauling.展开更多
Molecular dynamics simulations have been performed to investigate the structural properties of hydroxyl-substituted alkyl benzenesulfonate monolayers formed at the water/vapor and water/decane interfaces.We report a d...Molecular dynamics simulations have been performed to investigate the structural properties of hydroxyl-substituted alkyl benzenesulfonate monolayers formed at the water/vapor and water/decane interfaces.We report a detailed study of the interfacial properties-liquid density profile,hydrogen bond structure,surfactant aggregate structure and order parameter-of the novel anionic surfactant,sodium 2-hydroxy-3-decyl-5-octylbenzenesulfonate(C10C8OHphSO3Na).Simulation results show that:with increasing number of surfactant molecules,the average number of intramolecular hydrogen bonds per surfactant molecule in the monolayer decreases,but the structures forming the intramolecular hydrogen bonds still play a dominant role;the hydrophobic part of the alkyl tail chain,especially the decyl substituent on the third carbon atom in the benzene ring,becomes straighter,and more ordered towards the external interface at higher surfactant coverage;two-dimensional radial distribution functions can describe the characteristic of surfactant aggregate structures and highlight the decane phase effect on the orientation of the hydrophobic part of the surfactant;the surfactant molecules readily form long-range hydrogen bonded structures.Our results are an important complement to experimental studies.We used the all-atom model by employing the GROMACS and ffAMBER programs in the simulations,which provides a new way to simulate the interfacial behavior of alkyl benzenesulfonate surfactants.展开更多
In this paper, the application of molecular catalysis for steam reforming of ethanol （SRE） is reviewed. Eight metals （Ni, Co, Cu Pt, Rh, Pd, Ir and Ru） have shown high catalytic activity for SRE. Among them Ni and...In this paper, the application of molecular catalysis for steam reforming of ethanol （SRE） is reviewed. Eight metals （Ni, Co, Cu Pt, Rh, Pd, Ir and Ru） have shown high catalytic activity for SRE. Among them Ni and Rh are very promising because of high d character in the metal bond and low metal-oxygen bonding （vs. metal-carbon）. They can effectively promote C-C bond cleavage in the rate-determining process during SRE. However, Rh is weak in water-gas-shift so that CH4 and CO become the main by-products at low reaction temperatures, while Ni catalysts suffer from rapid deactivation due to coking and sintering. Two low-temperature CO-free catalysts have been developed in our lab, namely Rh-Fe/Ca-Al2O3 and carbonyl-derived Rh-Co/CeO2, in which the presence of iron oxide or Co can promote water-gas-shift reaction and significantly improve the SRE performance. On the other hand, adding 3 wt% CaO to Ni/Al2O3 can greatly improve the catalyst stability because the Ca modification not only increases Ni concentration on the Ni/Ca-Al2O3 surface and 3d valence electron density, but also facilitates the water adsorption and coke gasification via water-gas-shift. The availability of abundant surface OH groups helps the formation and conversion of adsorbed formate intermediate. Hence, ethanol reaction on Ca-Al2O3-supported Ni, Pt, Pd and Rh catalysts are found to follow the formate-intermediated pathway, a new reaction pathway alternative to the traditional acetate-interrnediated pathway.展开更多
基金Supported by the National Natural Science Foundation of China(21276076)the Program for New Century Excellent Talents in University(NCET-13-0801)the Fundamental Research Funds for the Central Universities(222201313011)
文摘Ni/Mg–Al catalysts derived from hydrotalcite-type precursors were prepared by a co-precipitation technique and applied to steam reforming of methane. By comparison with Ni/γ-Al2O3 and Ni/α-Al2O3 catalysts prepared by incipient wetness impregnation, the Ni/Mg–Al catalyst presented much higher activity as a result of higher specific surface area and better Ni dispersion. The Ni/Mg–Al catalyst with a Ni/Mg/Al molar ratio of 0.5:2.5:1 exhibited the highest activity for steam methane reforming and was selected for kinetic investigation. With external and internal diffusion limitations eliminated, kinetic experiments were carried out at atmospheric pressure and over a temperature range of 823–973 K. The results demonstrated that the overall conversion of CH4 and the conversion of CH4 to CO2were strongly influenced by reaction temperature, residence time of reactants as well as molar ratio of steam to methane. A classical Langmuir–Hinshelwood kinetic model proposed by Xu and Froment(1989)fitted the experimental data with excellent agreement. The estimated adsorption parameters were consistent thermodynamically.
文摘Adsorption equilibrium isotherms of benzene in the concentrationrange of 500-4000 mg·m^-3 on two commercial activated carbons wereobtained using long-column method under 30 deg. C and differenthumidity condi- tions. Results show that the benzene and water vaporshave depression effects upon the adsorption of each other and thatthe unfavorable effect of water vapor resembles its single-componentisotherm on activated carbon. A com- petitive adsorption model wasproposed to explore the depression mechanisms of the non-ideal,non-similar binary adsorption systems.
文摘We synthesized a mesoporous film based on TiO2-reduced graphene oxide(RGO)hybrids using a one-step vapor-thermal method without the need for an additional annealing process.The vapor-thermally prepared TiO2-graphene hybrid(VTH)features unique structures with an ultra-large specific surface area of^260 m^2 g^-1 and low aggregation,giving rise to enhanced light harvesting and increased charge generation and separation efficiency.It was observed that a mesoporous film with uniform pore distribution is simultaneously obtained during the VTH growth process.When a 5.0 wt%RGO VTH film was used as the active layer in photocatalysis,the highest photocatalytic activity for degradation of methyl orange was achieved.For another,when a 0.75 wt%RGO VTH film was used as the photoanode in a dye-sensitized solar cell,the power conversion efficiency reached 7.58%,which represents an increase of 73.1%compared to a solar cell using an a photoanode of pure TiO2 synthesized by a traditional solvothermal method.It is expected that this facile method for the synthesis of TiO2/graphene hybrid mesoporous films will be useful in practical applications for preparing other metal oxide/graphene hybrids with ultra-high photocatalytic activity and photovoltaic performance.
基金Projects(21376274,51206192)supported by the National Natural Science Foundation of China
文摘A simplified model was developed to describe the water vapor adsorption on activated carbon. The development of the simplified model was started from the original model proposed by DO and his co-workers. Two different kinds of carbon materials were prepared for water vapor adsorption, and the adsorption experiments were conducted at different temperatures(20-50 °C) and relative humidities(5%-99%) to test the model. It is shown that the amount of adsorbed water vapor in micropore decreases with the temperature increasing, and the water molecules form larger water clusters around the functional group as the temperature is up to a higher value. The simplified model describes reasonably well for all the experimental data. According to the fitted values, the parameters of simplified model were represented by the temperature and then the model was used to calculate the water vapor adsorption amount at 25 °C and 35 °C. The results show that the model can get relatively accurate values to calculate the water vapor adsorption on activated carbon.
基金Supported by the National Natural Science Foundation of China (No. 29976046) and the Major State Basic Research Program(G2000026403).
文摘The XG equation, which is developed by us previously for describing the adsorption equilibrium of pure vapor on activated carbon, is extended to multi-component system. Verified by experimental data, the extended XG equation was found to be more successful in predicting the adsorption equilibrium of vapor mixture on activated carbon than the extended Langmuir equation, the extended BET equation and the ideal adsorbed solution theory (IAST).
文摘This study was conducted to evaluate the effect of different distillation methods of Mentha cordifolia Opiz. essential oil on antibacterial activity. The essential oils were isolated by water and steam, hydro, ethanol, and 3methanol： lethanol distillations. Moreover, we also compared the efficacy of these various distillations with commercial peppermint oil. Essential oils were tested in vitro against three pathogen bacteria species by sensitivity test include disc diffusion assay （DD）, minimal inhibition concentration （MIC） and maximal bactericidal concentration （MBC）. Escherichia coli, Staphylococcus aureus and Salmonella typhimurium were used in this investigation. The results showed that the water and steam distillation and 3methanol： lethanol under tested by DD assay was found to be effective against all the pathogenic bacteria, in which the zone of inhibition exhibited E. coil S. aureus and S. typhimurium were 9.67 ± 0.35, 11.67 ± 0.66, 18.0± 1.15 and 9.00 ± 0.05, 8.3 ± 0.35, 19.0 ± 0.00 ram, respectively. While the hydro and ethanol distillations did action to against only E. coli which the inhibition zones were 8.67 ± 0.66 and 8.67 ± 0.35 mm, respectively. However, the commercial oil was more effective against tested pathogenic bacteria than all M. cordifolia essential oil. In case of MIC and MBC assays, the results showed that all essential oil distillation methods posed antibacterial potential in which the water and steam distillation showed the lowest MIC and MBC values against E. coli, S. aureus and S. typhimurium. It is suggested that among all M. cordifolia essential oil extractions, water and steam distillation was found to be highly bactericidal as it has shown in lowest MIC and MBC values and high in growth inhibition zone diameter.
基金Projects(21376274,51206192)supported by the National Natural Science Foundation of China
文摘Five different kinds of hydrophilic organic salts were used to modify commercial activated carbon in order to prepare hydrophilic carbon materials. Properties of the samples were analyzed by surface area analyzer and SEM-EDX. The hydrophilic organic salts with different properties were introduced into activated carbon and significantly affected the properties of the samples.During adsorption experiments, the water vapor adsorption amount in modified samples increases by 0.57-17.12 times in temperature range from 303 to 323 K and at relative pressure below 0.50. Water molecules combined with surface hydrophilic groups through H-bonding exhibit good thermo stability. The effects of temperature, oxygen content and properties of the hydrophilic organic salts on water vapor adsorption were studied. It is indicated that water vapor adsorption in modified samples is mainly affected by the surface oxygen content. The carboxylate radicals in the hydrophilic organic salts greatly affect the micropore structure of the modified samples, while the metal ions in them exhibit limited influence. Different adsorption capacity of modified samples can be explained with the electronegativity of elements presented by Pauling.
基金supported by the National Natural Science Foundation of China (21003143)
文摘Molecular dynamics simulations have been performed to investigate the structural properties of hydroxyl-substituted alkyl benzenesulfonate monolayers formed at the water/vapor and water/decane interfaces.We report a detailed study of the interfacial properties-liquid density profile,hydrogen bond structure,surfactant aggregate structure and order parameter-of the novel anionic surfactant,sodium 2-hydroxy-3-decyl-5-octylbenzenesulfonate(C10C8OHphSO3Na).Simulation results show that:with increasing number of surfactant molecules,the average number of intramolecular hydrogen bonds per surfactant molecule in the monolayer decreases,but the structures forming the intramolecular hydrogen bonds still play a dominant role;the hydrophobic part of the alkyl tail chain,especially the decyl substituent on the third carbon atom in the benzene ring,becomes straighter,and more ordered towards the external interface at higher surfactant coverage;two-dimensional radial distribution functions can describe the characteristic of surfactant aggregate structures and highlight the decane phase effect on the orientation of the hydrophobic part of the surfactant;the surfactant molecules readily form long-range hydrogen bonded structures.Our results are an important complement to experimental studies.We used the all-atom model by employing the GROMACS and ffAMBER programs in the simulations,which provides a new way to simulate the interfacial behavior of alkyl benzenesulfonate surfactants.
基金The funding from the Institute of Chemical and Engineering Sciences,Singapore,to support the project"Alcohol Reforming for Hydrogen Generation"
文摘In this paper, the application of molecular catalysis for steam reforming of ethanol （SRE） is reviewed. Eight metals （Ni, Co, Cu Pt, Rh, Pd, Ir and Ru） have shown high catalytic activity for SRE. Among them Ni and Rh are very promising because of high d character in the metal bond and low metal-oxygen bonding （vs. metal-carbon）. They can effectively promote C-C bond cleavage in the rate-determining process during SRE. However, Rh is weak in water-gas-shift so that CH4 and CO become the main by-products at low reaction temperatures, while Ni catalysts suffer from rapid deactivation due to coking and sintering. Two low-temperature CO-free catalysts have been developed in our lab, namely Rh-Fe/Ca-Al2O3 and carbonyl-derived Rh-Co/CeO2, in which the presence of iron oxide or Co can promote water-gas-shift reaction and significantly improve the SRE performance. On the other hand, adding 3 wt% CaO to Ni/Al2O3 can greatly improve the catalyst stability because the Ca modification not only increases Ni concentration on the Ni/Ca-Al2O3 surface and 3d valence electron density, but also facilitates the water adsorption and coke gasification via water-gas-shift. The availability of abundant surface OH groups helps the formation and conversion of adsorbed formate intermediate. Hence, ethanol reaction on Ca-Al2O3-supported Ni, Pt, Pd and Rh catalysts are found to follow the formate-intermediated pathway, a new reaction pathway alternative to the traditional acetate-interrnediated pathway.
